Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 30, Pages 9382-9386Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201804817
Keywords
electrocatalysis; graphdiyne; hydrogen evolution; platinum; single-atom catalysts
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Funding
- National Key R&D Program of China [2017YFA0700104]
- NSFC [21790052, 21331007, 21773288]
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Two Pt single-atom catalysts (SACs) of Pt-GDY1 and Pt-GDY2 were prepared on graphdiyne (GDY) supports. The isolated Pt atoms are dispersed on GDY through the coordination interactions between Pt atoms and alkynyl C atoms in GDY, with the formation of five-coordinated C-1-Pt-Cl-4 species in Pt-GDY1 and four-coordinated C-2-Pt-Cl-2 species in Pt-GDY2. Pt-GDY2 shows exceptionally high catalytic activity for the hydrogen evolution reaction (HER), with a mass activity up to 3.3 and 26.9 times more active than Pt-GDY1 and the state-of-the-art commercial Pt/C catalysts, respectively. Pt-GDY2 possesses higher total unoccupied density of states of Pt 5d orbital and close to zero value of Gibbs free energy of the hydrogen adsorption (|Delta GP(H)*(Pt)|) at the Pt active sites, which are responsible for its excellent catalytic performance. This work can help better understand the structure-catalytic activity relationship in Pt SACs.
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